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<p>Electrochemical urea synthesis from CO<sub>2</sub> and NO<sub>3</sub><sup>−</sup> provides a sustainable alternative to industrial processes, yet remains challenged by inefficient C-N coupling and protonation. Here, we present a tandem urea electrosynthesis pathway over copper-supported palladium hydride (PdH<sub>x</sub>/Cu) through a dual spillover of CO* and H*. This pathway undergoes efficient CO<sub>2</sub>-to-CO* conversion on PdH<sub>x</sub> and facile NO<sub>3</sub><sup>−</sup>-to-NO* conversion on Cu. Crucially, rapid spillover of CO* (from PdHx surface) and H* (from PdH<sub>x</sub> lattice) to Cu facilitates key C-N intermediate (OCNO*) formation and protonation, respectively. Our catalysts demonstrated high performance, achieving a urea production rate of 236.5 ± 8.9 mmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> with a Faradaic efficiency for urea of 62.6 ± 1.8%. With these catalysts, our scaled-up flow cell enabled continuous co-production of urea and formate with consistent profitability and much lower CO<sub>2</sub> emissions compared to these for the present-day urea production route. This achievement represents a significant step for sustainable urea production.</p>

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Dual spillover of carbon monoxide and hydrogen initiates tandem urea electrosynthesis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月7日

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  • Yuefei Li,
  • Bingying Han,
  • Yurong Liu,
  • Ye Liu,
  • Riguang Zhang,
  • Baojun Wang,
  • Yu Chen,
  • Bao Yu Xia,
  • Jiayuan Li

摘要

Electrochemical urea synthesis from CO2 and NO3− provides a sustainable alternative to industrial processes, yet remains challenged by inefficient C-N coupling and protonation. Here, we present a tandem urea electrosynthesis pathway over copper-supported palladium hydride (PdHx/Cu) through a dual spillover of CO* and H*. This pathway undergoes efficient CO2-to-CO* conversion on PdHx and facile NO3−-to-NO* conversion on Cu. Crucially, rapid spillover of CO* (from PdHx surface) and H* (from PdHx lattice) to Cu facilitates key C-N intermediate (OCNO*) formation and protonation, respectively. Our catalysts demonstrated high performance, achieving a urea production rate of 236.5 ± 8.9 mmol gcat−1 h−1 with a Faradaic efficiency for urea of 62.6 ± 1.8%. With these catalysts, our scaled-up flow cell enabled continuous co-production of urea and formate with consistent profitability and much lower CO2 emissions compared to these for the present-day urea production route. This achievement represents a significant step for sustainable urea production.